Nucleic acids are unique, informational molecules with exceptional potential in the preparation of complex nanostructured materials with utility as potent and specific therapeutic agents in vivo and as powerful investigative tools in vitro. See e.g., Winfree, E. et al., 1998 Nature 394:539-544; Akhtar, S. et al., 2000, Adv. Drug Deliv. Rev. 44:3-21; Thomas, M. & Klibanov, A. M., 2003, App. Microbiol. Biotechnol. 62:27-34; Davis, M., 2002, E. Curr. Opinion Biotechnol. 13:128-131. Despite this promise, unmodified nucleic acids are inherently susceptible to enzymatic degradation in biological milieu, limiting their practical utility in detection and as therapeutics in real-world applications. To mitigate these issues, considerable effort has been applied to the generation of DNA analogues capable of resisting attack. See e.g., Leumann, C. J., 2002, Bioorg. Med. Chem. 10:841-854; Eschenmoser, A., 2005, Chimia 59:836-850. However, an optimal approach would preserve the natural nucleic acid sequence and associated hybridization properties. Therefore, new approaches for the preparation of well-defined, stable and competent nucleic acid-based materials are required.